This paper presents a comparison of two-component ammonia-based inlet atmospheres diluted with either hydrogen (NH3/H2) or nitrogen (NH3/N2). Taking advantage of the features of inlet atmospheres diluted with nitrogen and hydrogen, four two-stage processes were designed and carried out, which were juxtaposed with two single-stage processes carried out only in an NH3 atmosphere. A common parameter of the processes carried out was the same value of nitrogen availability in each process stage. The gas nitriding process was carried out on ASIS 1085 non-alloy steel and ASIS 52100 alloy steel. It was found that the chemical composition of the steels studied, for the adopted nitriding process parameters, did not affect the kinetics of the growth in the mass of nitrided samples as a function of the nitriding time. However, the additions of alloying elements present in the steels studied significantly affected the nitrogen distribution between the resulting iron nitride layer and the diffusion zone in the nitrided substrate. Because of the presence of chromium in AISI 52100 steel, a larger mass of nitrogen accumulated in the nitriding zone in the solution compared with unalloyed AISI 1085 steel. As a result, with the same increase in the mass of nitrided steel, a thicker layer of iron nitrides formed on AISI 1085 steel than on AISI 52100 steel.